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Waste to Catalyst: Synthesis of Catalysts from Sewage Sludge of the Mining, Steel, and Petroleum Industries

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Waste to Catalyst: Synthesis of Catalysts from Sewage Sludge of the Mining, Steel, and Petroleum Industries sustainability Article Waste to Catalyst: Synthesis of Catalysts from Sewage Sludge of the Mining, Steel, and Petroleum Industries Gabriela Castro-León, Erik Baquero-Quinteros, Bryan G. Loor, Jhoselin Alvear, Diego E. Montesdeoca Espín, Andrés De La Rosa and Carolina Montero-Calderón * Chemical Engineering Faculty, Universidad Central del Ecuador, Ritter s/n & Bolivia, Quito 17-01-3972, Ecuador; [email protected] (G.C.-L.); [email protected] (E.B.-Q.); [email protected] (B.G.L.); [email protected] (J.A.); [email protected] (D.E.M.E.); [email protected] (A.D.L.R.) * Correspondence: [email protected] Received: 5 August 2020; Accepted: 22 September 2020; Published: 25 November 2020 Abstract: The generation of sewage sludge presents a problem for several manufacturing companies as it results from industrial processes or effluent treatment systems. The treatment of this type of waste requires high economic investment, for this reason, it is necessary to find alternatives to recover the valuable materials of the sludges. In this study, metal catalysts were synthesized using waste sludge from the steel, mining, and hydrocarbon industries. The waste sludge was subjected to thermal treatments for the removal of organic content and the reduction of metals with hydrogen current to activate their catalytic properties. The sludge and synthesized catalysts were analyzed to determine their physical, chemical, thermoenergetic, and catalytic properties. Catalytic activity was evaluated using CO chemisorption and by thermal–catalytic decomposition of crude oil. The best conditions for synthesizing the catalysts were a calcination temperature between 300 and 500 ◦C and a reduction temperature between 300 and 900 ◦C. The catalysts presented a specific surface between 2.33 and 16.78 m2/g. The catalytic material had a heat capacity between 0.7 and 1.2 kJ/kg K. The synthesized · materials presented catalytic activity comparable to that of commercial catalysts. With this recovery technique, the industrial waste can be valorized, obtaining catalyst derived from the sludges and promoting the circular economy of manufacturing companies. Keywords: sewage sludge; mining tailings; steelworks; oil tank bottoms; catalysts; waste valorization; circular economy 1. Introduction Global waste generation is expected to double by 2025, of which industrial waste will comprise nearly 50% of the total. Global waste generation is projected to reach 11 million tons/day by 2100 [1]. Production processes use raw materials based on metals or containing metals, and some wastes are generated as sludge in the production stages, which often cannot be minimized. These process sludges, as well as those generated in water treatment systems, are considered hazardous waste according to Ecuadorian regulations [2]; therefore, sludge must be technically disposed of through environmental management. In Ecuador in 2017, it was estimated that 300 thousand tons of sewage sludge was generated and that companies invested approximately $200 million in environmental prevention processes [3]. Thus, Ecuador seeks to promote sustainable production and responsible consumption alternatives that include the recovery of raw materials from waste as part of its new economic development agenda based on the circular economy [4]. The economic potential of organic sewage sludge valorization for biogas production, co-incineration, or as a fertilizer in landscaping and agriculture is considered to be a possible Sustainability 2020, 12, 9849; doi:10.3390/su12239849 www.mdpi.com/journal/sustainability Sustainability 2020, 12, 9849 2 of 16 line of action for the support of the social and solidarity economy of communities in developing countries [5]. Alternatives involving the encapsulation of sludge as a part of construction materials have been proposed, such as the incorporation of tailings from lead mine washing plants in ceramics for bricks [6], the use of gold mine tailings as cement mortar [7,8], and the preparation of high-porosity bricks by utilizing red mud and mine tailings [9]. Some recovery alternatives for the synthesis of chemicals for the retention of metal contaminants have been reported, such as the use of residuals from drinking water treatment as an adsorbent for the retention of phosphorus compounds [10], for metal removal from electroplating wastewater effluent [11], or the adsorption of heavy metal ions by porous material prepared with silicate tailings [12]. The recovery of metal components present in sludge includes the production of iron-based secondary raw material from bauxite tailings and red muds [13] and gold recovery from mining waste by thiosulphate leaching [14]. Sludges from the electroplating process have been used to produce inorganic pigments for applications in ceramic glazes [15], and kimberlite tailings have been used in carbon capture [16]. The synthesis of metal catalysts from sewage sludge and their application in the oxidation of hydrocarbons has been reported since 2000 [17]. Since then, similar applications have been reported for multiple purposes, such as the oxidative dehydrogenation of propane with textile sludge-based catalysts [18], for the removal of volatile organic compounds using ferric catalysts derived from sludge produced by water purification [19], and for the N H insertion reaction using catalysts derived from − sewage sludge of carbonaceous materials [20]. Our research group has studied catalytic activity in crude cracking reactions using a catalyst derived from sludge resulting from wastewater treatment by the textile [21], the galvanoplasty [22], and tannery [23] industries, obtaining yields comparable to those for commercial catalysts. These catalysts have also been tested in terms of the catalytic decomposition of methane [24], in which conversion rates of reactants higher than 90% were obtained. Due to this, materials that have part of the organic or polymeric matrix with oxides or metals [25,26] can be used as photocatalyst. This work evaluated the possibility of synthesizing catalysts from waste sludge from three industries with the potential for economic development in Ecuador: sludge from the wastewater treatment plants of steelworks, metal mining tailings, and tank bottom sludge from hydrocarbon storage. These sludges contain metals such as iron, gold, and copper that could confer catalytic properties. After synthesis, the physical, chemical, and thermoenergetic properties were characterized, and the catalytic capacity of the materials was determined. The catalysts derived from mining tailings presented good thermal stability and a catalytic activity comparable to commercial catalysts. This alternative method to valorize hazardous sludges could aid in the implementation of the national development plans based on the circular economy. 2. Results 2.1. Samples Identification The sludge samples were supplied by three different manufacturing companies located in Ecuador (Table1). Company 1, located in the south of Ecuador, is a mine tailing deposit where artisanal mining waste is collected. This company generates two types of sludge: aged tailings (S1) and fresh tailings (S2). Company 2, located in the center of Ecuador, is a steelwork facility where the residual sludge comes from its wastewater treatment plant (S3). Company 3 is located in the Amazon region of Ecuador, and the sludge (S4) is bottom waste from petroleum storage tanks. The catalytic materials derived from each of these sludges were identified as C1, C2, C3, and C4 (Figure1a–d). Sustainability 2020, 12, 9849 3 of 16 Sustainability 2020, 12, x FOR PEER REVIEW 3 of 16 Table 1. Nomenclature used for the different studied sludges. Table 1. Nomenclature used for the different studied sludges. Company Type of Sludge Sludge Catalytic Material 1aCompany AgedType mining of Sludge tailings Sludge S1 Catalytic Material C1 1b1a FreshAged mining mining tailingstailings S1 S2 C1 C2 21b WastewaterFresh sludge mining from tailings a steelwork S2 S3 C2 C3 32 BottomWastewater sludge from sludge petroleum from a steelwork storage tanks S3 S4 C3 C4 3 Bottom sludge from petroleum storage tanks S4 C4 (a) (b) (c) (d) FigureFigure 1. Dried1. Dried fresh fresh mine mine tailings tailings S1 ( aS1), aged(a), aged mine mine tailings tailings S2 (b), S2 wastewater (b), wastewater sludge sludge from a steelworkfrom a S3steelwork (c), and bottom S3 (c), sludgeand bottom from sludge petroleum from storagepetroleum tanks storage S4 (d tanks). S4 (d). 2.2.2.2. Catalyst Catalyst Preparation Preparation TheThe preparation preparation of of catalysts catalysts has has beenbeen describeddescribed in previous previous works works by by our our research research group group [21,22]. [21,22 ]. TheThe samples samples were were gradually gradually dried dried in in order order toto preventprevent damage to to their their porous porous structure. structure. At At the the same same time,time, temperatures temperatures and and calcination calcination timestimes werewere chosen based based on on the the metals metals present present in inthe the sludge, sludge, namelynamely Au Au [27 [27–29],–29], Fe Fe [30 [30–33],–33], and and Cu Cu [[29,34,35].29,34,35]. The range range of of calcination calcination te temperaturesmperatures was was selected selected accordingaccording to to the the possible possible metals metals containedcontained inin the samples to to avoid avoid metal metal sintering sintering due due to tohigh high temperatures.temperatures. The The conditions conditions for for sludge
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